Abstract
CH4 emissions from inland waters are highly uncertain in the current global CH4 budget, especially for streams, rivers, and other lotic systems. Previous studies have attributed the strong spatiotemporal heterogeneity of riverine CH4 to environmental factors such as sediment type, water level, temperature, or particulate organic carbon abundance through correlation analysis. However, a mechanistic understanding of the basis for such heterogeneity is lacking. Here, we combine sediment CH4 data from the Hanford reach of the Columbia River with a biogeochemical-transport model to show that vertical hydrologic exchange flows (VHEFs), driven by the difference between river stage and groundwater level, determine CH4 flux at the sediment-water interface. CH4 fluxes show a nonlinear relationship with the magnitude of VHEFs, where high VHEFs introduce O2 into riverbed sediments, which inhibit CH4 production and induce CH4 oxidation, and low VHEFs cause transient reduction in CH4 flux (relative to production) due to reduced advective CH4 transport. In addition, VHEFs lead to the hysteresis of temperature rise and CH4 emissions because high river discharge caused by snowmelt in spring leads to strong downwelling flow that offsets increasing CH4 production with temperature rise. Our findings reveal how the interplay between in-stream hydrologic flux besides fluvial-wetland connectivity and microbial metabolic pathways that compete with methanogenic pathways can produce complex patterns in CH4 production and emission in riverbed alluvial sediments.
| Original language | English |
|---|---|
| Pages (from-to) | 4014-4026 |
| Number of pages | 13 |
| Journal | Environmental Science and Technology |
| Volume | 57 |
| Issue number | 9 |
| DOIs | |
| State | Published - Mar 7 2023 |
| Externally published | Yes |
Funding
This study was supported by the National Key R&D program of China (No. 2021YFC3200502) and the National Natural Science Foundation of China (No. 42141003, No. 41931292). The computational resources for the model calculations were supported by the Center for Computational Science and Engineering at Southern University of Science and Technology. This research was also supported by the U.S. Department of Energy, Office of Biological and Environmental Research, Environmental System Science (ESS) program through grants DE-SC0016217 and DE-SC0020309. PNNL is operated for DOE by Battelle Memorial Institute under contract DE-AC05-76RL01830. This paper describes objective technical results and analysis. Any subjective views or opinions that might be expressed in the paper do not necessarily represent the views of the U.S. Department of Energy or the United States Government.
Keywords
- microbial-explicit model
- riverine CH emission
- sediment biogeochemical cycling
- temperature hysteresis
- vertical hydrologic exchange flows
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